Local coordination atom and metal types of single-atom catalysts to regulate catalytic performance of C2H2 selective hydrogenation

[Display omitted] •Local coordination atom and metal types can tune catalytic performance of SACs.•Local coordination atoms of SACs tune electronic properties of single-atom metal.•C2H4 activity has an inverted volcano relationship with d-band center in Co SACs.•Co-N3C presents high C2H4 selectivity and activity, and better stability.•C2H4 selectivity on Co SACs enhances with the increase of coordination atom electronegativity. The local coordination environment of anchoring single-atom metal is the design core of single-atom catalysts (SACs). In this study, several kinds of single-atom M (M = Co, Ni, Cu, Pt, Pd and Ru) anchored over the dual-coordination N and other heteroatom (B/C/N/O/S/P)-doped graphene catalysts (M-N3-B/C/N/O/S/P SACs) were theoretically predicted and indirectly supported by the reported experiment to tune catalytic performance of C2H2 selective hydrogenation. Co-N3C catalyst was screened out to exhibit high C2H4 selectivity and activity, and better stability in C2H2 selective hydrogenation. More electrons loss of single-atom Co corresponds to weaker C2H4 adsorption energy to improve C2H4 selectivity. Further, C2H4 activity has an inverted volcano relationship with d-band center in Co SACs. This work provides a theoretical basis to screen and design SACs with better structural stability and excellent catalytic performance by adjusting the local coordination atom and metal types of metal SACs.